甲烷水蒸气重整制氢研究进展 |
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| 3 甲烷水蒸气重整过程中催化剂的研究
甲烷水蒸气重整为吸热反应，通过热力学分析可知，该反应需要在高温、高水碳比、低压下进行，若没有催化剂参与，则该重整过程反应速率缓慢。因此，催化剂对于甲烷水蒸气重整制氢反应过程非常重要。 Dan等[72]采用共沉淀法制备了Ni/Al2O3、Ni/MgO-Al2O3、Ni/La2O3-Al2O3 3种催化剂应用于甲烷水蒸气重整过程，得出催化剂催化活性按照Ni/Al2O3＜Ni/La2O3-Al2O3≈Ni/MgO-Al2O3顺序排列。Kdor等[73]对Ni/Al2O3中掺杂Au的催化剂活性进行分析，结果表明，加入Au成分可以很好地抑制甲烷水蒸气重整反应中炭沉积的形成。Eunkyung等[74]对蛋壳型Ni负载在MgAl2O4催化剂进行研究，发现蛋壳型催化剂的稳定性与抗积炭能力比普通催化剂好。Lu等[75]对甲烷水蒸气在Ni/Al2O3、Ni/γ-Al2O3-MgO、Ni-CeO2/γ-Al2O3-MgO 3种催化剂上的重整反应过程进行研究，结果表明，Ni-CeO2/γ-Al2O3-MgO的催化效率最佳。Yu等[76]研究了采用共沉淀、溶胶-凝胶、醇解3种方法制备的Ni/MgAl2O4催化剂对甲烷水蒸气重整制氢过程的影响，结果表明，采用溶胶-凝胶法制备的催化剂具有较高的活性和抗积炭能力。Dmitry[77]模拟研究了甲烷水蒸气在经过预热的Ni基催化剂上的重整反应过程，得出催化剂床层在1 300 K时，反应中合成气组分达到平衡。Gao等[78]研究了甲烷水蒸气在Ni-Ce/ZSM-5催化剂上的重整反应，得出在该催化剂下甲烷转化率可达到95%，同时，该催化剂可以保持40 h的活性。Ambrosetti等[79]基于甲烷水蒸气在Rh/Al2O3催化剂表面进行的重整反应过程提出一种新的反应动力学，该动力学可以准确地表述甲烷水蒸气重整反应过程。Lee等[80]研究了甲烷水蒸气在Ni/K2TixOyAl2O3催化剂表面进行的反应，结果表明，与Ni/Al2O3相比，Ni/K2TixOyAl2O3催化剂的稳定性及抗积炭能力更好。Hiramitsu等[81]研究了甲烷水蒸气在蜂窝状纯镍催化剂表面进行重整反应，结果表明，重整过程可以使甲烷转化率达到97%，同时，催化剂表面几乎不会产生炭沉积。Yang等[82]对不同铈含量的Ni-Ce/Al2O3催化甲烷水蒸气重整过程进行研究，结果表明，在催化剂中添加含量合适的铈才具有最佳的催化性能。Wang等[83]开发出活性高、性能稳定、抗积炭能力强的Rh/MgO-Al2O3催化剂用于甲烷水蒸气重整反应。 综上所述，在甲烷部分氧化反应过程中贵金属的积炭量顺序为Pd>>Rh＞Ru＞Pt＞Ir。对于非贵金属Fe、Co、Ni负载于载体Al2O3上的催化剂，研究结果表明，Ni催化剂活性及抗积炭能力好。相比价格昂贵的贵金属催化剂，非贵金属催化剂在工业上应用广泛，虽然催化剂成分不同，但为了防止催化剂表面积炭，通常会在催化剂中加入某种助剂。因此，制备活性高、性能稳定、抗积炭能力强的催化剂成为甲烷水蒸气重整制氢的重要研究方向。 4 结论与展望甲烷水蒸气重整制氢作为一种有效的制氢方法，可以解决温室气体的排放与清洁能源获取的问题。甲烷水蒸气重整制取合成气在能源与环境方面具有重要意义。随着近年来研究的不断深入，甲烷水蒸气重整的实验方法与测试技术不断完善，其研究取得了很大进展，但对其反应机理仍存在很大的争议，今后的研究应基于热力学软件对甲烷水蒸气重整制氢过程的反应特性进行模拟计算，通过优化工况参数确定最佳反应条件，探索反应机理，为甲烷水蒸气重整的工业生产提供理论指导。对于甲烷水蒸气重整反应器的选择，在考虑成本的同时，还要得到高纯度的产物。此外，对于催化剂的研究应寻求操作方法简单、价格低廉、原料储量丰富、可以获得高活性材料的研究方法，并探求催化剂与化学反应之间的关系，进而制备出活性高、性能稳定、抗积炭能力强的催化剂，这是目前需要解决的主要问题。 参考文献 [1] ALTAMASH T, KHRAISHEH M, QURESHI M F. 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